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This chapter discusses recent experimental work exploring the optical properties and quantum dynamics of organic semiconductor nanostructures based on squaraine dyes. SquarainesSquaraines are prototypical quadrupolar charge-transfer chromophoresCharge-transfer chromophores of interest for solution-processed photovoltaics and as aggregates with large circular dichroism. Here, we demonstrate and exploit their unique properties as quantum emitters for implementing hybrid nanostructures featuring strong exciton-plasmon couplingsExciton-plasmon coupling. We show that the unusual electronic properties of squarainesSquaraines result in a substantial reduction of vibronic couplingVibronic coupling to the ubiquitous high-frequency C–C-bond-stretching modes of organic materials and in the formation of spectrally narrow J-aggregated exciton resonances in squaraine thin films. This is exploited to create metallic nanostructuresMetallic nanostructures covered with squaraine thin films and to perform the first time-domain study of coherent exciton-plasmon couplingsExciton-plasmon coupling using two-dimensional electronic spectroscopyTwo-dimensional electronic spectroscopy with 10-fs time resolution. The experiments present unexpected evidence for long-range coherent exciton transport driven by plasmonic fields. This opens up new opportunities for manipulating the coherent transport of matter excitations by coupling to vacuum fields.

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Two-Dimensional Electronic Spectroscopy of Organic Semiconductor Nanostructures

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  • 发表日期：

    2025年

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  • Daniel Timmer,
  • Christoph Lienau

摘要

This chapter discusses recent experimental work exploring the optical properties and quantum dynamics of organic semiconductor nanostructures based on squaraine dyes. SquarainesSquaraines are prototypical quadrupolar charge-transfer chromophoresCharge-transfer chromophores of interest for solution-processed photovoltaics and as aggregates with large circular dichroism. Here, we demonstrate and exploit their unique properties as quantum emitters for implementing hybrid nanostructures featuring strong exciton-plasmon couplingsExciton-plasmon coupling. We show that the unusual electronic properties of squarainesSquaraines result in a substantial reduction of vibronic couplingVibronic coupling to the ubiquitous high-frequency C–C-bond-stretching modes of organic materials and in the formation of spectrally narrow J-aggregated exciton resonances in squaraine thin films. This is exploited to create metallic nanostructuresMetallic nanostructures covered with squaraine thin films and to perform the first time-domain study of coherent exciton-plasmon couplingsExciton-plasmon coupling using two-dimensional electronic spectroscopyTwo-dimensional electronic spectroscopy with 10-fs time resolution. The experiments present unexpected evidence for long-range coherent exciton transport driven by plasmonic fields. This opens up new opportunities for manipulating the coherent transport of matter excitations by coupling to vacuum fields.